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The police action came a year after Albanian authorities banned such activities.
More than 1,500 police officers took part in the operation that took place in Tirana and seven other cities, while European League football matches took place on Thursday evening.
In a statement, police said have arrested 117 people and 24 others are being investigated.
“They are the owners, managers or employees of these bets. The police also seized 140,000 euros and hundreds of computers and other electronic devices,” the police statement said.
In 2018, Albania's parliament voted to abolish gambling in residential areas.
Casinos are now allowed only in some large hotels.
However, many such activities have continued to operate in secrecy.
Online betting sites are also illegal in Albanian cities.